Hydrogen Yield from CO2 Reforming of Methane: Impact of La2O3 Doping on Supported Ni Catalysts

Development of a transition metal based catalyst aiming at concomitant high activity and stability attributed to distinguished catalytic characteristics is considered as the bottleneck for dry reforming of methane (DRM). This work highlights the role of modifying zirconia (ZrO2) and alumina (Al2O3) supported nickel based catalysts using lanthanum oxide (La2O3) varying from 0 to 20 wt% during dry reforming of methane. The mesoporous catalysts with improved BET surface areas, improved dispersion, relatively lower reduction temperatures and enhanced surface basicity are identified after La2O3 doping. These factors have influenced the catalytic activity and higher hydrogen yields are found for La2O3 modified catalysts as compared to base catalysts (5 wt% Ni-ZrO2 and 5 wt% Ni-Al2O3). Post-reaction characterizations such as TGA have showed less coke formation over La2O3 modified samples. Raman spectra indicates decreased graphitization for La2O3 catalysts. The 5Ni-10La2O3-ZrO2 catalyst produced 80% hydrogen yields, 25% more than that of 5Ni-ZrO2. 5Ni-15La2O3-Al2O3 gave 84% hydrogen yields, 8% higher than that of 5Ni-Al2O3. Higher CO2 activity improved the surface carbon oxidation rate. From the study, the extent of La2O3 loading is dependent on the type of oxide support.

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Effects of the Mg addition on characteristics and catalytic activity of Ni/-Al2O3 in dry reforming of methane

Science and Technology Development Journal - Natural Sciences ◽

10.32508/stdjns.v1it5.538 ◽

2018 ◽

Vol 1 (T5) ◽

pp. 85-94

Author(s):

Loc Cam Luu ◽

Tri Nguyen ◽

Cuong Tien Hoang ◽

Tien Trong Nguyen ◽

Minh Hoang Phan ◽

...

Keyword(s):

Reaction Temperature ◽

Flow Reactor ◽

Coke Formation ◽

Dry Reforming ◽

Dry Reforming Of Methane ◽

Co2 Reforming ◽

Temperature Programmed Oxidation ◽

Co2 Reforming Of Ch4 ◽

Temperature Programmed ◽

Α Al2o3

Effectively using CO2-containing natural gas is an urgent requirement in Vietnam. Therefore, producing hydrogen and syngas by dry reforming of methane (СН4+СО2 = 2Н2+2СО) has gained renewed interest in recent years. In this paper, Ni/α- Al2O3 and Ni-Mg/α-Al2O3 catalysts were prepared by impregnation. Physico-chemical characteristics of catalysts were investigated via nitrogen physisorption (BET), X-Ray Diffraction (XRD), Transmission Electron Microscopy (TEM), and Temperature Programmed Reduction (TPR) methods. The activities of catalysts in CO2 reforming of CH4 were studied in a micro-flow reactor in the temperature range 550 –800oC, and content of CH4 and CO2 of 3 % mol. It was found that the conversion of CH4 and CO2 remarkably increased with the increase of reaction temperature from 550 to 700oC, but increased inconsiderably when the temperature reached more than 700oC. The selectivities of CO and H2 reached over 91 %. The modification of Ni/α- Al2O3 catalyst with Mg led to reduce the NiO particle size forme the new ZnO-MgO solid solution and increase the reductivity of catalyst. These improve the activity, selectivity and stability of catalyst. At the reaction temperature of 700oC, the conversions of CH4 and CO2 on Ni-Mg/α-Al2O3 reached 88.5 % and 72.3 %, respectively. The activities of catalysts were stable for 30 hours of reaction. Moreover, the role of Mg in the resistance to the coke formation on the catalyst surface was clarified via the results of temperature programmed oxidation (TPO) of spent catalysts after running the reaction for 30 hours at 700oC

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In Situ Elucidation of the Active State of Co–CeOx Catalysts in the Dry Reforming of Methane: The Important Role of the Reducible Oxide Support and Interactions with Cobalt

ACS Catalysis ◽

10.1021/acscatal.7b03640 ◽

2018 ◽

Vol 8 (4) ◽

pp. 3550-3560 ◽

Cited By ~ 34

Author(s):

Feng Zhang ◽

Zongyuan Liu ◽

Shuhao Zhang ◽

Nusnin Akter ◽

Robert M. Palomino ◽

...

Keyword(s):

Dry Reforming ◽

Active State ◽

Dry Reforming Of Methane ◽

Oxide Support

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Ni-Silica-based Catalysts for CH4 Reforming by CO2 with Enhanced Stability: Recent Designs and the Impacts of Ni Confinement, Promoters, and Core-Shell Structures

10.21926/jept.2101007 ◽

2021 ◽

Vol 3 (1) ◽

Author(s):

Oscar Daoura ◽

◽

Maya Boutros ◽

Franck Launay ◽

Keyword(s):

Heterogeneous Catalysts ◽

Catalyst Deactivation ◽

High Surface ◽

High Surface Area ◽

Dry Reforming ◽

Dry Reforming Of Methane ◽

Future Research ◽

Co2 Reforming ◽

Co2 Reforming Of Ch4 ◽

Oxide Support

CO2 reforming of CH4, also referred to as the Dry Reforming of Methane (DRM), is considered an excellent method to produce H2 and CO (syngas), which are known to be used for the production of higher alkanes and oxygenates. Despite nickel’s moderate toxicity, Ni-based heterogeneous catalysts are considered excellent candidates for use in DRM due to their reasonable performances and economic advantages. However, these materials also present severe drawbacks, such as sintering of the active phase and coke (carbon) deposition, which may, in certain cases, lead to severe catalyst deactivation. Several synthesis strategies, mostly based on the stabilization of nickel through oxide support, have been developed to overcome these issues. Silica-based materials are investigated widely due to their availability, high surface area, and the confinement capacity conferred by their controlled porosity. The present review summarizes the progress in the design of Ni/silica-based catalysts for the dry reforming of methane between the years 2015 and 2018. The different strategies implemented are discussed to assist future research works in designing the anti-coking and anti-sintering nickel-silica-based catalysts.

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Influence of Fe, La, Zr, Ce, and Ca on the catalytic performance and coke formation in dry reforming of methane over Ni/MgO.Al2O3 catalyst

Chemical Engineering Science ◽

10.1016/j.ces.2021.116956 ◽

2021 ◽

pp. 116956

Author(s):

Somaye Sadat Miri ◽

Fereshteh Meshkani ◽

Ali Rastegarpanah ◽

Mehran Rezaei

Keyword(s):

Coke Formation ◽

Catalytic Performance ◽

Dry Reforming ◽

Dry Reforming Of Methane

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Enhanced activity and stability of MgO-promoted Ni/Al2O3 catalyst for dry reforming of methane: Role of MgO

Fuel ◽

10.1016/j.fuel.2020.119082 ◽

2021 ◽

Vol 284 ◽

pp. 119082

Author(s):

Baitang Jin ◽

Shiguang Li ◽

Xinhua Liang

Keyword(s):

Dry Reforming ◽

Dry Reforming Of Methane ◽

Enhanced Activity ◽

Al2o3 Catalyst

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Atomically dispersed nickel as coke-resistant active sites for methane dry reforming

Nature Communications ◽

10.1038/s41467-019-12843-w ◽

2019 ◽

Vol 10 (1) ◽

Cited By ~ 46

Author(s):

Mohcin Akri ◽

Shu Zhao ◽

Xiaoyu Li ◽

Ketao Zang ◽

Adam F. Lee ◽

...

Keyword(s):

Active Sites ◽

Large Scale ◽

Low Cost ◽

Coke Formation ◽

Dry Reforming ◽

Dry Reforming Of Methane ◽

Highly Active ◽

Catalytic Sites ◽

Earth Abundant ◽

Poor Stability

AbstractDry reforming of methane (DRM) is an attractive route to utilize CO2 as a chemical feedstock with which to convert CH4 into valuable syngas and simultaneously mitigate both greenhouse gases. Ni-based DRM catalysts are promising due to their high activity and low cost, but suffer from poor stability due to coke formation which has hindered their commercialization. Herein, we report that atomically dispersed Ni single atoms, stabilized by interaction with Ce-doped hydroxyapatite, are highly active and coke-resistant catalytic sites for DRM. Experimental and computational studies reveal that isolated Ni atoms are intrinsically coke-resistant due to their unique ability to only activate the first C-H bond in CH4, thus avoiding methane deep decomposition into carbon. This discovery offers new opportunities to develop large-scale DRM processes using earth abundant catalysts.

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Dry Reforming of Methane over Ni–Al2O3 and Ni–SiO2 Catalysts: Role of Preparation Methods

Catalysis Letters ◽

10.1007/s10562-020-03120-3 ◽

2020 ◽

Vol 150 (8) ◽

pp. 2180-2199 ◽

Cited By ~ 2

Author(s):

S. Dekkar ◽

S. Tezkratt ◽

D. Sellam ◽

K. Ikkour ◽

K. Parkhomenko ◽

...

Keyword(s):

Dry Reforming ◽

Dry Reforming Of Methane ◽

Preparation Methods

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Investigation of Ce(iii) promoter effects on the tri-metallic Pt, Pd, Ni/MgO catalyst in dry-reforming of methane

RSC Advances ◽

10.1039/c5ra25869c ◽

2016 ◽

Vol 6 (13) ◽

pp. 10372-10384 ◽

Cited By ~ 18

Author(s):

Faris A. J. Al-Doghachi ◽

Umer Rashid ◽

Yun Hin Taufiq-Yap

Keyword(s):

Dry Reforming ◽

Hydrogen Gas ◽

The Other ◽

Methane Molecule ◽

Dry Reforming Of Methane ◽

Promoter Effects

The DRM reaction on the Pt, Pd, Ni/Mg1−XCeXO catalyst was studied where the methane molecule was activated on the Ni metal to produce hydrogen gas. The role of the other metals like Pt and Pd impregnated on the surface of the catalyst was shown.

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